Methylated nitrogenous heterocycles derived from pyridines, isoquinolines, Harmala alkaloids, pteridines, and related compounds are being metalated to afford novel carbanions. Subsequent condensations of such species with a variety of aldehydes, alkyl halides, esters, ketones, lactones, nitriles, and other electrophiles are expected to afford new compounds, some of which may have antineoplastic activity.